Evaluation of flumequine antibiotic removal from synthetic aqueous media using US / Fe-doped TiO2 process

Authors
1 Health Promotion Research Center, Zahedan University of Medical Sciences, Zahedan, Iran
2 Department of Natural Resources and Environment, Science and Research Branch, Islamic Azad University, Tehran, Iran
3 Faculty of Natural Sciences and Environment, Department of Environmental Engineering, Tehran Science and Research Branch, Islamic Azad University, Tehran, Iran
Abstract
Introduction

The use of antibiotics in veterinary medicine and medical applications has increased widely and the possibility of contamination of water sources with such compounds has increased which causes adverse effects such as increased bacterial resistance and digestive disorders. Therefore, the aim of this study was to use the ultrasonic process with Fe-doped TiO2 nano-particle in the Removal of flumequine.

Materials and Methods

The present study was an experimental-laboratory study conducted as a batch system. nanoparticles were synthesized by the sol-gel method and SEM, XRD, and DRS analyzes were used to determine the properties of nanoparticles. The effect of different variables including pH (3-11), initial concentration of flumequine (25-75 mg/L), and concentration of nanoparticles (200-600 mg/L) at different times (15-60 min) Was examined in sonocatalytic removal of flumequine.

Results

The results of this study showed that the maximum removal efficiency of flumequine was 96.5 % at pH 3, initial concentration of 25 mg/L, and a nanoparticle dose of 600 mg/L, a reaction time of 60 minutes was obtained using ultrasonic waves with a constant frequency of 35 kHz.

Conclusion

Due to the high removal efficiency of sonocatalytic process, the use of this process for the removal of flumequine in water and wastewater treatment processes is recommended.
Keywords

1. Xu W-h, Zhang G, Zou S-c, Li X-d, Liu Y-c. Determination of selected antibiotics in the Victoria Harbour and the Pearl River, South China using high-performance liquid chromatography-electrospray ionization tandem mass spectrometry. Environ Pollut. 2007;145(3):672-9.
2. Dehghani S, JONIDI JA, Farzadkia M, Gholami M. Investigation of the efficiency of Fenton’s advanced oxidation process in sulfadiazine antibiotic removal from aqueous solutions. Arak Med. Univ. J. 2012; 15(66): 19-29. (persian).
3. Kitazono Y, Ihara I, Yoshida G, Toyoda K, Umetsu K. Selective degradation of tetracycline antibiotics present in raw milk by electrochemical method. J Hazard Mater. 2012; 243:112-6.
4. Clarke BO, Smith SR. Review of ‘emerging’organic contaminants in biosolids and assessment of international research priorities for the agricultural use of biosolids. Environ Int. 2011;37(1):226-47.
5. Rodayan A, Roy R, Yargeau V. Oxidation products of sulfamethoxazole in ozonated secondary effluent. J Hazard Mater. 2010;177(1-3):237-43.
6. Xian Q, Hu L, Chen H, Chang Z, Zou H. Removal of nutrients and veterinary antibiotics from swine wastewater by a constructed macrophyte floating bed system. J Environ Manage. 2010;91(12):2657-61.
7. Zuccato E, Castiglioni S, Bagnati R, Melis M, Fanelli R. Source, occurrence and fate of antibiotics in the Italian aquatic environment. J Hazard Mater. 2010;179(1-3):1042-8.
8. Fink L, Dror I, Berkowitz B. Enrofloxacin oxidative degradation facilitated by metal oxide nanoparticles. Chemosphere. 2012;86(2):144-9.
9. Wu S, Zhao X, Li Y, Zhao C, Du Q, Sun J, et al. Adsorption of ciprofloxacin onto biocomposite fibers of graphene oxide/calcium alginate. Chem Eng J. 2013; 230:389-95.
10. Ji Y, Ferronato C, Salvador A, Yang X, Chovelon J-M. Degradation of ciprofloxacin and sulfamethoxazole by ferrous-activated persulfate: implications for remediation of groundwater contaminated by antibiotics. Sci Total Environ. 2014; 472:800-8.
11. Esplugas S, Bila DM, Krause LGT, Dezotti M. Ozonation and advanced oxidation technologies to remove endocrine disrupting chemicals (EDCs) and pharmaceuticals and personal care products (PPCPs) in water effluents. J Hazard Mater. 2007;149(3):631-42.
12. Gutiérrez M, Grillini V, Mutavdžić Pavlović D, Verlicchi P. Activated carbon coupled with advanced biological wastewater treatment: A review of the enhancement in micropollutant removal. Sci Total Environ. 2021; 790:148050.
13. Zhu T-t, Su Z-x, Lai W-x, Zhang Y-b, Liu Y-w. Insights into the fate and removal of antibiotics and antibiotic resistance genes using biological wastewater treatment technology. Sci Total Environ. 2021;776:145906.
14. Ye W-K, Tian F-X, Xu B, Zhao D-S, Ye J, Wang B, et al. Insights into the enhanced degradation of flumequine by UV/ClO2 integrated process: Kinetics, mechanisms and DBPs-related toxicity in post-disinfection. Sep Purif Technol. 2022; 280:119846.
15. Lloret L, Eibes G, Lú-Chau T, Moreira M, Feijoo G, Lema J. Laccase-catalyzed degradation of anti-inflammatories and estrogens. Biochem Engin J. 2010;51(3):124-31.
16. Bautitz IR, Nogueira RFP. Degradation of tetracycline by photo-Fenton process—Solar irradiation and matrix effects. J Photochem Photobio A: Chem. 2007;187(1):33-9.
17. Mohammadi AS, Attar HM. P-chlorophenol oxidation in industrial effluent by ultrasonic/fenton technology. Water Wastewater. 2011;22(4):80.
18. Zhang H, Wei C, Huang Y, Wang J. Preparation of cube micrometer potassium niobate (KNbO 3) by hydrothermal method and sonocatalytic degradation of organic dye. Ultrason sonochem. 2016; 30:61-9.
19. Tabasideh S, Maleki A, Shahmoradi B, Ghahremani E, McKay G. Sonophotocatalytic degradation of diazinon in aqueous solution using iron-doped TiO2 nanoparticles. Sep Purif Technol. 2017; 189:186-92.
20. Moradi V, Jun MB, Blackburn A, Herring RA. Significant improvement in visible light photocatalytic activity of Fe doped TiO2 using an acid treatment process. Appl Surf Sci. 2018; 427:791-9.
21. Sui Y, Liu Q, Jiang T, Guo Y. Synthesis of nano-TiO2 photocatalysts with tunable Fe doping concentration from Ti-bearing tailings. Appl Surf Sci. 2018; 428:1149-58.
22. Lin L, Wang H, Jiang W, Mkaouar AR, Xu P. Comparison study on photocatalytic oxidation of pharmaceuticals by TiO2-Fe and TiO2-reduced graphene oxide nanocomposites immobilized on optical fibers. J Hazard Mater. 2017; 333:162-8.
23. Panda D, Manickam S. Recent advancements in the sonophotocatalysis (SPC) and doped-sonophotocatalysis (DSPC) for the treatment of recalcitrant hazardous organic water pollutants. Ultrason sonochem. 2017; 36:481-96.
24. Rehman S, Ullah R, Butt A, Gohar N. Strategies of making TiO2 and ZnO visible light active. J Hazard Mater. 2009;170(2-3):560-9.
25. Fei J, Li J. Controlled preparation of porous TiO2–Ag nanostructures through supramolecular assembly for plasmon‐enhanced photocatalysis. Adv Mater. 2015;27(2):314-9.
26. Norabadi E, Ashrafi SD, Kamani H, Jahantiq A. Degradation of 2,6-dichlorophenol by Fe-doped TiO2 Sonophotocatalytic process: kinetic study, intermediate product, degradation pathway. Int J Environ Anal Chem. 2020:1-16.
27. Nieto J, Freer J, Contreras D, Candal RJ, Sileo EE, Mansilla HD. Photocatalyzed degradation of flumequine by doped TiO2 and simulated solar light. J Hazard Mater. 2008;155(1-2):45-50.
28. Kamani H, Ashrafi SD, Jahantiq A, Norabadi E, Dashti Zadeh M. Catalytic degradation of humic acid using Fe–doped TiO2 - ultrasound hybrid system from aqueous solution. Int J Environ Anal Chem. 2021:1-15.
29. Norabadi E, Kord Mostafapour F, Kamani H, Bazrafshan E, Ashrafi SD, pirasteh k, et al. Photocatalytic process using magnesium oxide nanoparticles for amoxicillin removal from aqueous solution. J Torbat Heydariyeh Univ Med Sci. 2018;6(3):1-12. (persian).
30. Choi J, Park H, Hoffmann MR. Effects of single metal-ion doping on the visible-light photoreactivity of TiO2. J Phys Chem C Nanomater Interfaces. 2009;114(2):783-92.
31. Eadi SB, Kim S, Jeong SW, Jeon HW. Novel Preparation of Fe Doped TiO2 Nanoparticles and Their Application for Gas Sensor and Photocatalytic Degradation. Adv Mater Sci Eng. 2017;2017.
32. Farhangi N, Chowdhury RR, Medina-Gonzalez Y, Ray MB, Charpentier PA. Visible light active Fe doped TiO2 nanowires grown on graphene using supercritical CO2. Appl Catal B. 2011; 110:25-32.
33. Kamani H, Nasseri S, Khoobi M, Nodehi RN, Mahvi AH. Sonocatalytic degradation of humic acid by N-doped TiO 2 nano-particle in aqueous solution. J Environ Health Sci Eng. 2016;14(1):3.
34. Li J, Xu J, Dai W-L, Li H, Fan K. Direct hydro-alcohol thermal synthesis of special core–shell structured Fe-doped titania microspheres with extended visible light response and enhanced photoactivity. Appl Catal B. 2009;85(3):162-70.
35. Liu L, Chen F, Yang F, Chen Y, Crittenden J. Photocatalytic degradation of 2,4-dichlorophenol using nanoscale Fe/TiO2. Chem Eng J. 2012;181-182(Supplement C):189-95.
36. Reddy DR, Dinesh GK, Anandan S, Sivasankar T. Sonophotocatalytic treatment of Naphthol Blue Black dye and real textile wastewater using synthesized Fe doped TiO2. Chem Eng Process. 2016;99(Supplement C):10-8.
37. Sui Y, Liu Q, Jiang T, Guo Y. Synthesis of nano-TiO2 photocatalysts with tunable Fe doping concentration from Ti-bearing tailings. Appl Surf Sci. 2018;428(Supplement C):1149-58.
38. Pang YL, Abdullah AZ. Effect of low Fe3+ doping on characteristics, sonocatalytic activity and reusability of TiO2 nanotubes catalysts for removal of Rhodamine B from water. J Hazard Mater. 2012; 235:326-35.
39. Li XZ, Fan CM, Sun YP. Enhancement of photocatalytic oxidation of humic acid in TiO2 suspensions by increasing cation strength. Chemosphere. 2002;48(4):453-60.
40. Kamani H, Bazrafshan E, Ashrafi SD, Sancholi F. Efficiency of sono-nano-catalytic process of TiO2 nano-particle in removal of erythromycin and metronidazole from aqueous solution. J Mazandaran Univ Med Sci. 2017;27(151):140-54. (persian).
41. Verma A, Kaur H, Dixit D. Photocatalytic, Sonolytic and Sonophotocatalytic Degradation of 4-Chloro-2-Nitro Phenol. Arch Environ Protec 2013;39(2):17-28. Doi: 10.2478/aep-2013-0015
42. Qi Y, Qu R, Liu J, Chen J, Al-Basher G, Alsultan N, et al. Oxidation of flumequine in aqueous solution by UV-activated peroxymonosulfate: Kinetics, water matrix effects, degradation products and reaction pathways. Chemosphere. 2019; 237:124484.
43. Garcia-Segura S, Garrido JA, Rodríguez RM, Cabot PL, Centellas F, Arias C, et al. Mineralization of flumequine in acidic medium by electro-Fenton and photoelectro-Fenton processes. Water Res. 2012;46(7):2067-76.
44. Guo H, Jiang N, Wang H, Shang K, Lu N, Li J, et al. Degradation of flumequine in water by pulsed discharge plasma coupled with reduced graphene oxide/TiO2 nanocomposites. Sep Purif Technol. 2019; 218:206-16.
45. Gul I, Sayed M, Shah NS, Ali Khan J, Polychronopoulou K, Iqbal J, et al. Solar light responsive bismuth doped titania with Ti3+ for efficient photocatalytic degradation of flumequine: Synergistic role of peroxymonosulfate. Chem Eng J. 2020; 384:123255.
46. Iqbal J, Shah NS, Sayed M, Muhammad N, Rehman S-u, Khan JA, et al. Deep eutectic solvent-mediated synthesis of ceria nanoparticles with the enhanced yield for photocatalytic degradation of flumequine under UV-C. J Water Proc Eng. 2020;33:101012.
47. Lops C, Ancona A, Di Cesare K, Dumontel B, Garino N, Canavese G, et al. Sonophotocatalytic degradation mechanisms of Rhodamine B dye via radicals generation by micro- and nano-particles of ZnO. Appl Catal B. 2019; 243:629-40.
48. Mohammadi R, Massoumi B, Rabani M. Photocatalytic decomposition of amoxicillin trihydrate antibiotic in aqueous solutions under UV irradiation using Sn/TiO2 nanoparticles. Int. J. Photoenergy. 2012;2012.
49. Khan MAN, Siddique M, Wahid F, Khan R. Removal of reactive blue 19 dye by sono, photo and sonophotocatalytic oxidation using visible light. Ultrason Sonochem. 2015;26(Supplement C):370-7.
50. Sohrabnezhad S. Study of catalytic reduction and photodegradation of methylene blue by heterogeneous catalyst. Spectrochim Acta A Mol Biomol Spectrosc. 2011;81(1):228-35.
51. Hoseini M, Safari GH, Kamani H, Jaafari J, Ghanbarain M, Mahvi AH. Sonocatalytic degradation of tetracycline antibiotic in aqueous solution by sonocatalysis. Toxicol Environ Chem. 2013;95(10):1680-9.
52. ElShafei GM, Al-Sabagh A, Yehia F, Philip C, Moussa N, Eshaq G, et al. Metal oxychlorides as robust heterogeneous Fenton catalysts for the sonophotocatalytic degradation of 2-nitrophenol. Appl Catal B. 2018; 224:681-91.
53. Tabasideh S, Maleki A, Shahmoradi B, Ghahremani E, McKay G. Sonophotocatalytic degradation of diazinon in aqueous solution using iron-doped TiO2 nanoparticles. Sep Purif Technol. 2017;189(Supplement C):186-92.
54. Gad-Allah TA, Ali MEM, Badawy MI. Photocatalytic oxidation of ciprofloxacin under simulated sunlight. J Hazard Mater. 2011;186(1):751-5.
55. Hassani A, Khataee A, Karaca S, Karaca C, Gholami P. Sonocatalytic degradation of ciprofloxacin using synthesized TiO2 nanoparticles on montmorillonite. Ultrason Sonochem. 2017; 35:251-62.